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Title: Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”

We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit T H by cooling micrometer-sized droplets (microdroplets) evaporatively at 10³-10⁴ K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water's diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at <227 K, but vitrify at cooling rates of 10⁶–10⁷ K/s. We also hypothesize that the slower increase in the nucleation rate is connected with the proposed "fragile-to-strong" transition anomaly in water.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [5] ;  [1] ;  [1] ;  [1] ;  [6] ;  [7] ;  [7] ;  [1] ;  [8] ;  [1] ;  [1] ;  [9] ;  [10] ;  [5] ;  [11] more »;  [3] « less
  1. SLAC National Accelerator Laboratory, Menlo Park, CA (United States)
  2. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); Stockholm Univ., Stockholm (Sweden)
  4. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); National Univ. of Singapore, (Singapore)
  5. Stockholm Univ., Stockholm (Sweden)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States); Institue for Methods and Instrumentation in Synchrotron Radiation Research, Berlin (Germany)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  8. SLAC National Accelerator Laboratory, Menlo Park, CA (United States); National Science FOundation BioXFEL Science and Technology Center, Buffalo, NY (United States)
  9. Stockholm Univ., Stockholm (Sweden); Univ. of Innsbruck, Innsbruck (Austria)
  10. Univ. of Innsbruck, Innsbruck (Austria)
  11. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
OSTI Identifier:
1198682
Grant/Contract Number:
AC03-76SF00515
Type:
Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 14; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; homogeneous ice nucleation; supercooled water; diffusivity; fragile to strong liquid transition; X-ray free-electron laser